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First-Principles Modeling of Chlorine Isotope Fractionation Between First-principles modeling of chlorine isotope fractionation between chloride-bearing molecules and minerals Etienne Balan, Laura Créon, Chrystèle Sanloup, Jérôme Aléon, Marc Blanchard, Lorenzo Paulatto, Hélène Bureau To cite this version: Etienne Balan, Laura Créon, Chrystèle Sanloup, Jérôme Aléon, Marc Blanchard, et al.. First- principles modeling of chlorine isotope fractionation between chloride-bearing molecules and minerals. Chemical Geology, Elsevier, 2019, 525, pp.424-434. 10.1016/j.chemgeo.2019.07.032. hal-02326016 HAL Id: hal-02326016 https://hal.archives-ouvertes.fr/hal-02326016 Submitted on 8 Nov 2020 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. 1 2 3 First-principles modeling of chlorine isotope fractionation between 4 chloride-bearing molecules and minerals 5 6 7 Etienne Balan1, Laura Créon1, Chrystele Sanloup1, Jérôme Aléon1, Marc Blanchard2, 8 Lorenzo Paulatto1, Hélène Bureau1 9 10 11 12 1Sorbonne Université, CNRS, IRD, MNHN, Institut de Minéralogie, de Physique des Matériaux et de 13 Cosmochimie (IMPMC), 4 place Jussieu, 75252 Paris cedex 05, France 14 2Géosciences Environnement Toulouse (GET), Observatoire Midi-Pyrénées, Université de Toulouse, CNRS, 15 IRD, UPS, 14 avenue E. Belin, 31400 Toulouse, France 16 17 18 19 20 Keywords : Cl isotopes, first-principles modeling, brines, Cl-bearing minerals, solar 21 nebula 22 Abstract 23 24 Equilibrium 37Cl/35Cl fractionation factors in selected molecules, Cl-bearing 25 crystalline solids, and silicates in which Cl occurs at trace or minor concentration level 26 are determined from first-principles calculations, within the density functional theory 27 (DFT) scheme. Results on benchmarking molecules and crystalline solids are consistent 28 with the previous theoretical study of Schauble et al. (2003). The present study further 29 documents the control of the isotopic fractionation properties of chlorine by its local 30 bonding environment. Chloromagnesite and chlorapatite display similar isotopic 31 fractionation properties due to relatively similar bonding environment. In contrast, 32 trace Cl in Mg-serpentine (lizardite) and Mg-amphibole (anthophyllite) are enriched in 33 37Cl with respect to chloromagnesite, due to the structural constraints exerted by the 34 host structure on the substituted ion. This effect is even more pronounced when Cl is 35 associated to hydroxylated cationic vacancies in forsterite. An effect of the local bonding 36 environment on the Cl isotopic fractionation properties is also inferred for Cl- ions in 37 saturated aqueous solutions. It explains the systematic departure between theoretical 38 and empirical reduced partition function ratio observed for the alkaline chlorides, 39 differing from the agreement observed for the hydrated Cl salts. The reduced partition 40 function ratio of Cl- ions in concentrated solution of alkaline chlorides is smaller from 41 that observed in dilute solutions by an amount potentially reaching 1‰ at 22°C. Finally, 42 the calculation of fractionation factors between gas (HCl(g), NaCl(g), KCl(g)) and solids 43 (sodalite, chlorapatite, halite, HCl trihydrate) which likely prevailed in the solar nebula, 37 44 sustains a model in which the Cl enrichment of HCl(g) is produced by a Rayleigh type 45 fractionation during chlorine condensation at temperatures between 400 and 500 K. 46 This model could explain the heavier isotopic composition observed for bulk Earth and 47 various chondrites compared to the nebular gas. 48 49 1. Introduction 50 51 The 37Cl/35Cl isotopic composition of chlorine in major Earth's reservoirs 52 (seawater, evaporites, mantle) exhibits a limited range of values, with most of them 53 falling between -0.5 ‰ and +0.5 ‰ from the seawater composition (Eggenkamp, 2014; 54 Barnes and Sharp, 2017). Strong departures from these values are most often ascribed 55 to non-equilibrium kinetic processes affecting the Cl isotopic composition, which include 56 Cl loss during degassing processes (Sharp et al., 2010a,b) as well as diffusion and ion 57 filtration in porous media explaining negative values of sedimentary pore fluids (e.g. 58 Godon et al., 2004). At a larger scale, degassing processes are expected to explain the 59 heavier isotopic composition of planetary reservoirs, such as the Moon or the crust of 60 Mars, because of the preferential loss of light chlorine isotope (Sharp et al., 2010a; 61 Barnes and Sharp, 2017; Wang et al., 2019). Equilibrium isotopic fractionation of 62 chlorine in nature is generally expected to be of smaller magnitude because chlorine 63 mostly occurs under a single redox state, the reduced chloride ions, and the relative 64 mass difference between the isotopes is small. In addition, and although equilibrium 65 isotopic fractionation involving oxidized forms of chlorine such as perchlorates can be 66 large (Schauble et al., 2003), the photochemical formation of these unstable species is 67 not expected to fractionate the chlorine isotopes (Barnes and Sharp, 2017). 68 Few equilibrium fractionation factors of Cl isotopes have been experimentally - - 69 determined. They include the HCl-Cl (aq), (Sharp et al., 2010b) and the Cl2-Cl (aq) (Giunta et 70 al., 2017) fractionation coefficients at near-ambient conditions; as well as fractionation 71 between chloride salts and saturated solutions (Eggenkamp et al., 1995, 2016). At high 72 temperature, Sharp et al. (2007) reported a -0.3 ‰ fractionation factor between 73 sodalite and NaCl(l) at 825 °C and Cisneros (2013) documented a +0.1 ‰ fractionation 74 factor between amphibole and NaCl-bearing solution at 700°C and 0.2 GPa. Observations 75 made on seafloor serpentinite and altered oceanic crust also point to a small positive - - 76 serpentine-Cl (aq) and amphibole-Cl (aq) fractionation. 77 Theoretical isotopic fractionation factors between molecular species and 78 crystalline chlorides have been predicted by combining experimentally observed 79 vibrational frequencies and theoretically predicted frequency shifts due to the isotopic 80 substitution (Schauble et al., 2003). For molecules, theoretical predictions were based 81 on ab-initio quantum-mechanical calculations, whereas those for crystalline solids made 82 use of empirical force-fields. This set of theoretical fractionation coefficients revealed 83 significant equilibrium enrichment in 37Cl in oxidized chlorine species as well as in Cl- 84 bearing organic molecules. The fractionation between more reduced Cl2 and HCl 85 molecules was found to be consistent with experimental data and the role of the local 86 environment of chloride ions in minerals was underlined, suggesting enrichment of 87 silicates in 37Cl with respect to simple Na, K or Rb chlorides (Schauble et al., 2003). More 88 recently, Schauble and Sharp (2011) reported a -0.7 ‰ fractionation between sodalite 89 and HCl at 950 K and a -0.02 ‰ fractionation between sodalite and NaCl(c) at 1098 K. 90 They also predicted a +3 to +6 ‰ fractionation between crystalline HCl hydrate and 91 HCl(g) at 140-160 K, a fractionation potentially explaining the variability of Cl isotopic 92 composition observed in chondrites (Sharp et al., 2013; Gargano et al., 2017). 93 Previous studies have shown that theoretical fractionation factors computed 94 from first-principles within density functional theory (DFT) provide useful information 95 on isotopic systems that are difficult to address on a purely experimental basis because 96 they involve, e.g., uncommon isotopic effects (Schauble et al., 2006), slow chemical 97 reactions (Méheut et al., 2007), weakly fractionating isotopes (Blanchard et al., 2009; 98 Moynier et al., 2011; Blanchard et al., 2017), incorporation of minor or trace elements in 99 minerals (Rustad and Zarzycki, 2008; Balan et al., 2018) or high-temperature reactions 100 between solids and dilute gas (Javoy et al., 2012). In the present work, we apply this 101 approach to chlorine isotopes by providing a set of theoretical fractionation factors 102 between selected molecules (Table 1) and crystalline solids (Table 2) in which chlorine 103 occurs as a major or a trace element, all systems being treated at the same theoretical 104 level. This study mostly focuses on chloride, the lowest redox state of chlorine, which 105 corresponds to the most frequently observed in natural systems. The investigated 106 phases include cosmochemically important molecules, (HCl(g), NaCl(g) and KCl(g)), Cl- 107 bearing minerals (chlorapatite, sodalite, chloromagnesite and Cl salts precipitating from 108 aqueous solutions), as well as rock-forming silicates displaying Cl as a trace element 109 (lizardite, anthophyllite, forsterite). 110 111 2. Methods 112 113 2.1. Expression of isotopic fractionation factors 114 115 Assuming a system with two stable isotopes, the equilibrium isotopic 116 fractionation coefficient of an element Y between two phases a and b, referred to as 117 α(a,b,Y), is defined by the isotopic ratios: 118 119 α(a,b,Y)=(Y*/Y')a/(Y*/Y')b (1) 120 121 where Y* and Y' are the abundances of the two different isotopes. Accordingly,
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